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Physical Review A

Ambiguous resonances in multipulse quantum sensing with nitrogen-vacancy centers

Lucas Tsunaki, Anmol Singh, Kseniia Volkova, Sergei D. Trofimov, Tommaso Pregnolato, Tim Schröder, Boris Naydenov

Published Feb 7, 2025• 8 citations
Publisher

Abstract

Dynamical decoupling multipulse sequences can be applied to solid-state spins for sensing weak oscillating fields from nearby single nuclear spins. By periodically reversing the probing system's evolution, other noises are counteracted and filtered out over the total evolution. However, the technique is subject to intricate interactions resulting in additional resonant responses, which can be misinterpreted with the actual signal intended to be measured. We experimentally characterize three of these effects present in single nitrogen-vacancy centers in diamond, where we also develop a numerical simulation model without rotating-wave approximation, showing robust correlation to the experimental data. Regarding centers with the N 15 nitrogen isotope, we observe that a small misalignment in the bias magnetic field causes the precession of the nitrogen nuclear spin to be sensed by the electronic spin of the center. Another studied case of ambiguous resonances comes from the coupling with lattice C 13 nuclei, where we use the echo modulation frequencies to obtain the interaction Hamiltonian and then utilize the latter to simulate multipulse sequences. Finally, we also measure and simulate the effects from the free evolution of the quantum system during finite pulse durations. Due to the large data volume and the strong dependence of these ambiguous resonances with specific experimental parameters, we provide a simulations data set with a user-friendly graphical interface, where users can compare simulations with their own experimental data for spectral disambiguation. Although focused on nitrogen-vacancy centers and dynamical decoupling sequences, these results and the developed model can potentially be applied to other solid-state spins and quantum sensing techniques.

DOI
10.1103/physreva.111.022606

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Dynamical decoupling multipulse sequences can be applied to solid-state spins for sensing weak oscillating fields from nearby single nuclear spins. By periodically reversing the probing system's evolution, other noises are counteracted and filtered out over the total evolution. However, the technique is subject to intricate interactions resulting in additional resonant responses, which can be misinterpreted with the actual signal intended to be measured. We experimentally characterize three of these effects present in single nitrogen-vacancy centers in diamond, where we also develop a numerical simulation model without rotating-wave approximation, showing robust correlation to the experimental data. Regarding centers with the N 15 nitrogen isotope, we observe that a small misalignment in the bias magnetic field causes the precession of the nitrogen nuclear spin to be sensed by the electronic spin of the center. Another studied case of ambiguous resonances comes from the coupling with lattice C 13 nuclei, where we use the echo modulation frequencies to obtain the interaction Hamiltonian and then utilize the latter to simulate multipulse sequences. Finally, we also measure and simulate the effects from the free evolution of the quantum system during finite pulse durations. Due to the large data volume and the strong dependence of these ambiguous resonances with specific experimental parameters, we provide a simulations data set with a user-friendly graphical interface, where users can compare simulations with their own experimental data for spectral disambiguation. Although focused on nitrogen-vacancy centers and dynamical decoupling sequences, these results and the developed model can potentially be applied to other solid-state spins and quantum sensing techniques.
Quantum sensors based on the electron spin states of nitrogen vacancy centers in diamond have found wide application in magnetometry and nuclear spin magnetic resonance measurements. Previously, we have theoretically and experimentally investigated the effect of finite pulse width on quantum sensing for synchronous alternating-current (AC) magnetic fields to dynamical decoupling sequences [T. Ishikawa et al., Phys. Rev. Appl. 10, 054059 (2018)]. However, many biological and condensed-matter systems exhibit fluctuating AC fields over time, and thus, our model needs modifications because of additional non-ideal conditions in practical measurements. Here, we investigate the effects of finite pulse width of multiple-pulse decoupling sequences on quantum sensing for asynchronous AC magnetic fields. For this purpose, we use a spin ensemble of nitrogen vacancy centers in an isotopically purified diamond film. We reveal through experiments that the finite-width pulse causes shifts in AC magnetometry signals in a free-precession-time plot. In addition, our results indicate that the finite-width pulse affects the amplitude of magnetometry signals, implying that the finite-pulse-width effect should be taken into account for realizing accurate measurement of the frequency and amplitude of asynchronous AC magnetic fields.
We present a method to identify spurious signals generated by finite-width pulses in quantum sensing experiments and apply it to recently proposed dynamical decoupling sequences for accurate spectral interpretation. We first study the origin of these fake resonances and quantify their behavior in a situation that involves the measurement of a classical magnetic field. Here we show that a change of the initial phase of the sensor or, equivalently, of the decoupling pulses leads to oscillations in the spurious signal intensity while the real resonances remain intact. Finally we extend our results to the quantum regime for the unambiguous detection of remote nuclear spins by utilization of a nitrogen vacancy sensor in diamond.
Abstract A nitrogen-vacancy (NV) center in a diamond enables the access to an electron spin, which is expected to present highly sensitive quantum sensors. Although exploiting a nitrogen nuclear spin improves the sensitivity, manipulating it using a resonant pulse requires a long gate time owing to its small gyromagnetic ratio. Another technique to control nuclear spins is a conditional rotation gate based on dynamical decoupling, which is faster but unavailable for nitrogen spins owing to the lack of transverse hyperfine coupling with the electron spin. In this study, we generated effective transverse coupling by applying a weak off-axis magnetic field. An effective coupling depends on the off-axis field; the conditional rotation gate on the nitrogen-14 spins of an NV center was demonstrated within 4.2 μs under an 1.8% off-axis field and a longitudinal field of approximately 280 mT. We estimated that a population transfer from the electron to nitrogen spins can be implemented with 8.7 μs. Our method is applicable to an ensemble of NV centers, in addition to a single NV center.
Sensing, localizing, and identifying individual nuclear spins or frequency components of a signal in the presence of a noisy environment requires the development of robust and selective methods of dynamical decoupling. An important challenge that remains to be addressed in this context are spurious higher-order resonances in current dynamical decoupling sequences as they can lead to the misidentification of nuclei or of different frequency components of external signals. Here we overcome this challenge with engineered quantum sensing sequences that achieve both enhanced robustness and the simultaneous suppression of higher-order-harmonic resonances. We experimentally demonstrate the principle using a single nitrogen-vacancy center spin sensor which we apply to the unambiguous detection of external protons.
Characteristic dips appear in the coherence traces of a probe qubit when dynamical decoupling (DD) is applied in synchrony with the precession of target nuclear spins, forming the basis for nanoscale nuclear magnetic resonance (NMR). The frequency of the microwave control pulses is chosen to match the qubit transition but this can be detuned from resonance by experimental errors, hyperfine coupling intrinsic to the qubit, or inhomogeneous broadening. The detuning acts as an additional static field which is generally assumed to be completely removed in Hahn echo and DD experiments. Here we demonstrate that this is not the case in the presence of finite pulse-durations, where a detuning can drastically alter the coherence response of the probe qubit, with important implications for sensing applications. Using the electronic spin associated with a nitrogen-vacancy center in diamond as a test qubit system, we analytically and experimentally study the qubit coherence response under CPMG and XY8 dynamical decoupling control schemes in the presence of finite pulse-durations and static detunings. Most striking is the splitting of the NMR resonance under CPMG, whereas under XY8 the amplitude of the NMR signal is modulated. Our work shows that the detuning error must not be neglected when extracting data from quantum sensor coherence traces.
We develop theoretically and demonstrate experimentally a universal dynamical decoupling method for robust quantum sensing with unambiguous signal identification. Our method uses randomization of control pulses to simultaneously suppress two types of errors in the measured spectra that would otherwise lead to false signal identification. These are spurious responses due to finite-width π pulses, as well as signal distortion caused by π pulse imperfections. For the cases of nanoscale nuclear-spin sensing and ac magnetometry, we benchmark the performance of the protocol with a single nitrogen vacancy center in diamond against widely used nonrandomized pulse sequences. Our method is general and can be combined with existing multipulse quantum sensing sequences to enhance their performance.